His latest one-off, Broken Bells, could be his biggest stretch yet: It pairs him with career introvert James Mercer, the sublimely melodic singer-songwriter of the Shins. The two have a little history — one track together on Dark Night — but Mercer might seem an odd match for the producer whose first big idea was combining the Beatles with Jay-Z, and whose trademark move is melding hip-hop-rooted samples and beats with vintage psychedelia.

It turns out the two pop-science geeks are a perfect match. Danger Mouse pushes Mercer's gorgeous, existential tunecraft outward with Day-Glo dynamics. "'Cause they know, and so do I/The high road is hard to find," Mercer sings on the opening chorus of Bells. The lyrics are about the loneliness of decision-making — they may refer to life in the trenches of normalcy, or, perhaps, to Mercer's recent professional decisions (he more or less fired two members of the Shins). But what sweeps you up are the sweet, ascending verses, the rolling chorus and the Danger Mouse touches: analog-synth swirls, slo-mo kick drums, a melancholy bass line — hip-hop for turned-on shut-ins.

Cool variations on the Gnarls formula — Danger and a quirkily excellent singer making arty, transcultural pop — run throughout the album. "Vaporize" begins with Mercer's fey workaday voice and a strummed acoustic, then takes off with smeared snares, bouncy organ and a jaunty Bacharach-David-style horn break. It's punchier than the Shins, and livelier than you'd expect from a song whose title suggests innovative marijuana consumption — an anthem of solidarity for malcontents, teenage and otherwise, not unlike "Crazy." The catchy, midtempo "The Ghost Inside" even has Mercer singing in a T-Pained falsetto — it's not hard to imagine it on the hit parade, along with the soaring, U2-flavored "October."

Broken Bells isn't all crossover ambition. Tracks like "Your Head Is on Fire" — a drum-machine space waltz floating between Syd Barrett and something from Brian Eno's Another Green World — won't make the short list of Glee covers. But with a new Shins record reportedly brewing, Mercer seems to be following some of the instructions in his own songs: Life is short, brother — go for it. The introverted indie guy isn't gone, and he's still not afraid to tell you that we're ultimately alone on this journey. "If you want to follow me, you should know," he sings. "I was lost then/And I'm lost now/And I doubt I'll ever know which way to go." Maybe. But for the moment, in Danger Mouse, Mercer has found a promising fellow traveler.

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